EP1194481A1 - Resin compositions, method of producing resin compositions and filler blends for use in resin compositions - Google Patents
Resin compositions, method of producing resin compositions and filler blends for use in resin compositionsInfo
- Publication number
- EP1194481A1 EP1194481A1 EP99956367A EP99956367A EP1194481A1 EP 1194481 A1 EP1194481 A1 EP 1194481A1 EP 99956367 A EP99956367 A EP 99956367A EP 99956367 A EP99956367 A EP 99956367A EP 1194481 A1 EP1194481 A1 EP 1194481A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- microsilica
- talc
- filler
- resin compositions
- weight
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- 239000000945 filler Substances 0.000 title claims abstract description 48
- 239000000203 mixture Substances 0.000 title claims abstract description 35
- 239000011342 resin composition Substances 0.000 title claims abstract description 19
- 238000000034 method Methods 0.000 title claims abstract description 13
- 229910021487 silica fume Inorganic materials 0.000 claims abstract description 65
- 239000000454 talc Substances 0.000 claims abstract description 59
- 229910052623 talc Inorganic materials 0.000 claims abstract description 59
- 229920005992 thermoplastic resin Polymers 0.000 claims abstract description 31
- 239000004800 polyvinyl chloride Substances 0.000 claims abstract description 29
- 229920000915 polyvinyl chloride Polymers 0.000 claims abstract description 27
- 239000004952 Polyamide Substances 0.000 claims abstract description 20
- 229920002647 polyamide Polymers 0.000 claims abstract description 20
- 229920000098 polyolefin Polymers 0.000 claims abstract description 11
- 238000004519 manufacturing process Methods 0.000 claims abstract description 7
- 229920005989 resin Polymers 0.000 claims abstract description 3
- 239000011347 resin Substances 0.000 claims abstract description 3
- 150000001875 compounds Chemical class 0.000 claims description 3
- CHBRHODLKOZEPZ-UHFFFAOYSA-N Clotiazepam Chemical compound S1C(CC)=CC2=C1N(C)C(=O)CN=C2C1=CC=CC=C1Cl CHBRHODLKOZEPZ-UHFFFAOYSA-N 0.000 claims 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 16
- 229920001903 high density polyethylene Polymers 0.000 description 14
- 239000004700 high-density polyethylene Substances 0.000 description 14
- 239000004743 Polypropylene Substances 0.000 description 11
- -1 polypropylene Polymers 0.000 description 11
- 229920001155 polypropylene Polymers 0.000 description 11
- 238000013329 compounding Methods 0.000 description 7
- 229920000642 polymer Polymers 0.000 description 7
- 238000003490 calendering Methods 0.000 description 5
- 239000000377 silicon dioxide Substances 0.000 description 5
- 230000000052 comparative effect Effects 0.000 description 4
- 229910052500 inorganic mineral Inorganic materials 0.000 description 4
- 239000011707 mineral Substances 0.000 description 4
- 235000010755 mineral Nutrition 0.000 description 4
- 229920005606 polypropylene copolymer Polymers 0.000 description 3
- 229910052681 coesite Inorganic materials 0.000 description 2
- 229910052906 cristobalite Inorganic materials 0.000 description 2
- 229920006379 extruded polypropylene Polymers 0.000 description 2
- 239000010881 fly ash Substances 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 239000011164 primary particle Substances 0.000 description 2
- 229910052682 stishovite Inorganic materials 0.000 description 2
- 229920002725 thermoplastic elastomer Polymers 0.000 description 2
- 229910052905 tridymite Inorganic materials 0.000 description 2
- 229920011532 unplasticized polyvinyl chloride Polymers 0.000 description 2
- 229920000459 Nitrile rubber Polymers 0.000 description 1
- 239000004793 Polystyrene Substances 0.000 description 1
- 229910000676 Si alloy Inorganic materials 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- 229920006097 Ultramide® Polymers 0.000 description 1
- 229920000122 acrylonitrile butadiene styrene Polymers 0.000 description 1
- 229910021486 amorphous silicon dioxide Inorganic materials 0.000 description 1
- 229920001577 copolymer Polymers 0.000 description 1
- 229920001971 elastomer Polymers 0.000 description 1
- 239000000806 elastomer Substances 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
- 239000012767 functional filler Substances 0.000 description 1
- 238000001746 injection moulding Methods 0.000 description 1
- VTHJTEIRLNZDEV-UHFFFAOYSA-L magnesium dihydroxide Chemical compound [OH-].[OH-].[Mg+2] VTHJTEIRLNZDEV-UHFFFAOYSA-L 0.000 description 1
- 239000000347 magnesium hydroxide Substances 0.000 description 1
- 229960000816 magnesium hydroxide Drugs 0.000 description 1
- 229910001862 magnesium hydroxide Inorganic materials 0.000 description 1
- 235000012254 magnesium hydroxide Nutrition 0.000 description 1
- HCWCAKKEBCNQJP-UHFFFAOYSA-N magnesium orthosilicate Chemical compound [Mg+2].[Mg+2].[O-][Si]([O-])([O-])[O-] HCWCAKKEBCNQJP-UHFFFAOYSA-N 0.000 description 1
- 239000000391 magnesium silicate Substances 0.000 description 1
- 229910052919 magnesium silicate Inorganic materials 0.000 description 1
- 235000019792 magnesium silicate Nutrition 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 229920002492 poly(sulfone) Polymers 0.000 description 1
- 229920000058 polyacrylate Polymers 0.000 description 1
- 239000004417 polycarbonate Substances 0.000 description 1
- 229920000515 polycarbonate Polymers 0.000 description 1
- 229920000728 polyester Polymers 0.000 description 1
- 229920002223 polystyrene Polymers 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 229920006013 termoplastic resin Polymers 0.000 description 1
- 239000012808 vapor phase Substances 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/34—Silicon-containing compounds
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/34—Silicon-containing compounds
- C08K3/36—Silica
Definitions
- Resin compositions Method of producing resin compositions and filler blends for use in resin compositions.
- the present invention relates to new and improved resin compositions and more particularly to thermoplastic resin compositions such as polyolefines, polyvinylchloride and polyamide, and to a method for the production of resin compositions.
- the invention further relates to a filler blend for use in the production of resin compositions.
- polyolefines such as polypropylene compound containing functional fillers such as fine particulate talc to increase the stiffness of the final polypropylene product.
- Talc is hydrated magnesium silicate with the theoretical formula 3MgO.4SiO .H 2 O and consists of magnesiumhydroxide sandwiched between two sheets of silica.
- thermoplastic resin used in the specification and claims includes not only thermoplastic resins per se, but also mixtures thereof, as well as a blend of thermoplastic resins with other materials such as an elastomer like nitrile rubber.
- thermoplastic rubbers, thermoplastic elastomers are also included in the definition of thermoplastic resin.
- Thermoplastic resins per se includes polyolefines, polystyrene, polyesters, ABS copylymers, polyvinyl chloride (PVC), unplasticized polyvinyl chloride (UPVC), polyamide, acrylic polymers, polycarbonate polymers, polysulfone polymers and others.
- microsilica used in the specification and claims is particulate amorphous SiO 2 obtained from a process in which silica is reduced and the reduction product is oxidized in vapor phase to form amorphous silica.
- Microsilica may contain at least 70 % by weight silica (SiO 2 ) and have a specific density of 2,1 - 2.3 g/cm 3 and a surface area at 15 - 30 m 2 /g.
- the primary particles are substantially spherical.
- the primary particles have an average size of about 0,15 ⁇ m.
- Microsilica is preferably obtained as a co- product in the production of silicon or silicon alloys in electric reduction furnaces. In these processes large quantities of silica are formed as SiO 2 .
- microsilica also shall be understood to include fly-ash, and more particularly fly-ash particles of substantial spherical shape having a particle size below 10 microns.
- thermoplastic resin compositions particularly polyolefines, polyvinylchloride and polyamide, characterized in that the thermoplastic resin compositions contains between 3 and 400 % by weight of filler based on the weight of the resin, said filler comprising talc and microsilica where the weight ratio between talc and microsilica is between 15:1 and 1 :15.
- the weight ratio of talc and microsilica is between 6:1 and 1 :5.
- the present invention relates to a method for the production of thermoplastic resin composition, particularly polyolefines, polyvinylchloride and polyamide, which method being characterized in that talc and microsilica is added to thermoplastic resin in a total amount between 3 and 400 % by weight based on the weight of thermoplastic resin and where the weight ratio between talc and microsilica is kept between 15:1 and 1 :15, whereafter the mixture is formed into a thermoplastic resin product or compound.
- talc and microsilica are added to the thermoplastic resin as a mixture of talc and microsilica.
- the compounding of the termoplastic resin can be done using conventional processes like extrusion, calendering, injection moulding and others.
- the present invention relates to a filler blend for use in thermoplastic resins, particularly polyolefines, polyvinylchloride and polyamide, wherein the filler blend contains talc and microsilica in a weight ratio between 15:1 and 1 :15, and particularly between 6:1 and 1 :5. It has surprisingly been found that the combined use of talc and microsilica as fillers in thermoplastic resins, particularly in polyolefines, polyvinylchloride and polyamide, give final products having both high stiffness and high impact strength.
- a non-filled polypropylene copolymer "BA 202E" supplied by Borealis was extruded in a compounding extruder with addition of a filler blend consisting of talc supplied by Mondo Minerals OY and microsilica supplied by Elkem ASA.
- the weight ratio between talc and microsilica in the filler blend was 2:1 and tests were run with addition of 5,10 and 19 % by weight of the filler blend based on the weight of the polypropylene copolymer.
- the stiffness of the extruded polypropylene was measured as tensile modulus according to ISO 527 and the impact strength of the extruded polypropylene was measured as notched charpy impact strength according to ISO 179/1 A.
- the polypropylene copolymer was extruded in the compounding extruder with no addition of filler and with the addition 5, 10 and 18 % by weight of talc and with 5 and 10 % by weight of microsilica. Also for these comparative tests the stiffness and the impact strength were measured as stated above. The resulting stiffness and impact strength are shown in figure 1 and figure 2 respectively.
- the impact strength of the polypropylene containing both talc and microsilica is much higher than for the polypropylene containing only talc and only slightly lower than for the polypropylene containing only microsilica as a filler.
- the stiffness of the polypropylene containing both talc and microsilica is much higher than for polypropylene containing only microsilica as a filler and only slightly lower than for polypropylene containing only talc as a filler.
- the use of a blend of talc and microsilica thus surprisingly gives a polypropylene having both a high stiffness and a high impact strength.
- HDPE high density polyethylene copolymer
- HE 2467-BL A non-filled high density polyethylene copolymer "HDPE HE 2467-BL" supplied by Borealis was extruded in a compounding extruder with additon of a filler blend consisting of talc supplied by Mondo Minerals OY and microsilica supplied by Elkem ASA.
- the stiffness of the extruded HDPE was measured as tensile modulus according to ISO 527 and the impact strength of the extruded HDPE was measured as notched charpy impact strength according to ISO 179/1 A.
- the HDPE copolymer was extruded in the compounding extruder with no addition of filler, with the addition 10 % by weight of talc and with addition of 10 % by weight of microsilica. Also for these comparative tests the stiffness and the impact strength were measured as stated above. The resulting stiffness and impact strength are shown in table 1.
- the impact strength of the HDPE containing both talc and microsilica is higher than for the HDPE containing only talc, but lower than for the HDPE containing only microsilica as a filler.
- the stiffness of the HDPE containing both talc and microsilica is much higher than for HDPE containing only microsilica as a filler and only slightly lower than for HDPE containing only talc as a filler.
- the use of a blend of talc and microsilica thus surprisingly resulting in a HDPE having both a high stiffness and a high impact strength.
- a non-filled polyvinylchloride (PVC) polymer was calendered with additon of a filler blend consisting of talc supplied by Mondo Minerals OY and microsilica supplied by Elkem ASA.
- the weight ratio between talc and microsilica in the filler blend was 2:1 in one run and 1 :2 in another run, and the tests were run with addition of 5 % by weight of the filler blend based on the weight of PVC polymer.
- the stiffness of the calendered PVC was measured as tensile modulus according to ISO 527 and the impact strength of the calendered PVC was measured as notched charpy impact strength according to ISO 179/1 A.
- the impact strength of PVC containing talc and microsilica in a ratio of 2:1 is about the same as for the PVC containing only talc, but lower than for PVC containing only microsilica as a filler.
- PVC containing talc and microsilica in a ratio of 1 :2 it can be seen that the impact strength is higher than for PVC containing talc and microsilica in a ratio of 2:1 and almost as high as for PVC containing only microsilica.
- the stiffness of the PVC containing talc and microsilica in a ratio of 2:1 is much higher than for
- PVC containing only microsilica as a filler and only slightly lower than for PVC containing only talc as a filler.
- PVC containing only talc and microsilica in a ratio of 1 :2 it will be seen that the tensile modulus is still higher than for PVC containing only microsilica.
- the use of a blend of talc and microsilica thus surprisingly gives a PVC having both a high stiffness and a high impact strength.
- a non filled polyamide (PA) polymer, "PA6 Ultramid B35" delivered by BASF was extruded in a compounding extruder with addition of a filler blend consisting of talc supplied by Mondo Minerals OY and microsilica supplied by Elkem ASA.
- the addition of filler blend was 10 % by weight of polymer.
- the weight ratio between talc and microsilica in the filler blend in a first test was 1 :1 and 1 :2 in a the second test.
- the stiffness of the extruded PA was measured as tensile modulus according to ISO 527 and the impact strength of the extruded PA was measured as notched charpy impact strength according to ISA 179/1 A.
- the PA copolymer was extruded in the compounding extruder with no addition of filler, with the addition 10 % by weight of talc and with addition of 10 % by weight of microsilica. Also for these comparative tests the stiffness and the impact strength were measured as stated above. The resulting stiffness and impact strength are shown in table 3.
- the impact strength of the PA containing both talc and microsilica is much higher than for the PA containing only talc, but lower than for the PA containing only microsilica as a filler. It can also be seen that the impact strength increases with increasing amount of microsilica in the filler blend.
- the stiffness of the PA containing both talc and microsilica is much higher than for PA containing only microsilica, but the stiffness is slightly reduced when the microsilica content in the filler blend is increased.
Abstract
Description
Claims
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
NO985211A NO309484B1 (en) | 1998-11-09 | 1998-11-09 | Resin Compositions and Process for Preparing Resin Compositions |
NO985211 | 1998-11-09 | ||
PCT/NO1999/000336 WO2000027911A1 (en) | 1998-11-09 | 1999-11-08 | Resin compositions, method of producing resin compositions and filler blends for use in resin compositions |
Publications (2)
Publication Number | Publication Date |
---|---|
EP1194481A1 true EP1194481A1 (en) | 2002-04-10 |
EP1194481B1 EP1194481B1 (en) | 2005-08-10 |
Family
ID=19902604
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP99956367A Expired - Lifetime EP1194481B1 (en) | 1998-11-09 | 1999-11-08 | Resin compositions, method of producing resin compositions and filler blends for use in resin compositions |
Country Status (17)
Country | Link |
---|---|
US (1) | US6809144B1 (en) |
EP (1) | EP1194481B1 (en) |
JP (1) | JP3709342B2 (en) |
KR (1) | KR100407717B1 (en) |
CN (1) | CN1134493C (en) |
AT (1) | ATE301687T1 (en) |
AU (1) | AU1299100A (en) |
BR (1) | BR9915156A (en) |
CA (1) | CA2349489C (en) |
CZ (1) | CZ298481B6 (en) |
DE (1) | DE69926664T2 (en) |
ES (1) | ES2247839T3 (en) |
HU (1) | HU227716B1 (en) |
NO (2) | NO309484B1 (en) |
PL (1) | PL196537B1 (en) |
RU (1) | RU2201425C2 (en) |
WO (1) | WO2000027911A1 (en) |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US7197060B2 (en) | 2003-05-02 | 2007-03-27 | Videojet Technologies | Waveguide laser |
Families Citing this family (14)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
NO328601B1 (en) | 2002-06-07 | 2010-03-29 | Elkem As | Elastomeric compositions, process for the preparation of elastomeric compositions and the use of microsilica as a modifier in elastomeric compositions |
JP2004149635A (en) * | 2002-10-29 | 2004-05-27 | Daimaru Sangyo Kk | Polyolefin resin composition and method for producing the same |
NO328520B1 (en) * | 2004-11-03 | 2010-03-08 | Elkem As | Polyamide plastic with high flame resistance and good processability |
US20070037461A1 (en) * | 2005-08-09 | 2007-02-15 | Mondo S.P.A. | Laminar covering material |
NO325706B1 (en) * | 2006-02-15 | 2008-07-07 | Elkem As | Composite plastic material |
CN100392013C (en) * | 2006-05-15 | 2008-06-04 | 新疆大学 | Polyvinyl chloride organic smectite composite material and preparation process thereof |
US20090159170A1 (en) * | 2007-12-21 | 2009-06-25 | Karen Elaine Burkholder | Tire with innerliner containing low structure silica |
WO2010040359A1 (en) * | 2008-10-08 | 2010-04-15 | Vestas Wind Systems A/S | A method of manufacturing a polymer composite member by use of two or more resins |
NO330921B1 (en) * | 2008-10-15 | 2011-08-15 | Elkem As | Flame retardant polymeric materials |
EP2216350B1 (en) | 2009-02-04 | 2012-04-25 | Borealis AG | Polypropylene composition with high stiffness and impact strength |
EP2618339A3 (en) * | 2010-03-12 | 2013-10-30 | General Cable Technologies Corporation | Cable having insulation with micro oxide particles |
RU2447105C1 (en) * | 2010-11-24 | 2012-04-10 | Открытое акционерное общество "Институт пластмасс имени Г.С. Петрова" | Thermoplastic, scratch-resistant polymer composition |
CN103772966A (en) * | 2013-12-24 | 2014-05-07 | 贵州蓝图新材料有限公司 | Micro-silica fume reinforced nylon material and preparation method thereof |
KR101612429B1 (en) | 2015-05-04 | 2016-04-15 | 주식회사 브러시월드 | Resin Composition Using Biomass |
Family Cites Families (10)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4140669A (en) * | 1977-12-30 | 1979-02-20 | General Electric Company | Warp-resistant reinforced thermoplastic compositions comprising polyester resins, talc and silica |
US4722952A (en) * | 1986-05-09 | 1988-02-02 | Elkem A/S | Resin compositions |
GB2210882A (en) * | 1986-10-30 | 1989-06-21 | Bio Kil Chemicals Ltd | Settable composition suitable for lining pipes and sewers |
JPS63199253A (en) * | 1987-02-13 | 1988-08-17 | Shin Etsu Chem Co Ltd | Rubber composition |
GB2210826B (en) | 1987-10-19 | 1992-08-12 | Bowater Packaging Ltd | Barrier packaging materials |
US4956404A (en) * | 1989-01-10 | 1990-09-11 | Josef Pelzig | Plastic composition for toys, novelty items and arts and crafts |
US5266609A (en) * | 1989-01-27 | 1993-11-30 | Hall Neil R | Dental restorative adhesive having improved fracture toughness |
JP3501549B2 (en) | 1995-06-12 | 2004-03-02 | 王子製紙株式会社 | Thermal recording medium |
US5844037A (en) * | 1996-07-24 | 1998-12-01 | The Dow Chemical Company | Thermoplastic polymer compositions with modified electrical conductivity |
DE19645732A1 (en) * | 1996-11-06 | 1998-05-07 | Basf Ag | Powdery polymer compositions |
-
1998
- 1998-11-09 NO NO985211A patent/NO309484B1/en not_active IP Right Cessation
-
1999
- 1999-11-08 DE DE69926664T patent/DE69926664T2/en not_active Expired - Lifetime
- 1999-11-08 ES ES99956367T patent/ES2247839T3/en not_active Expired - Lifetime
- 1999-11-08 US US09/830,860 patent/US6809144B1/en not_active Expired - Fee Related
- 1999-11-08 WO PCT/NO1999/000336 patent/WO2000027911A1/en active IP Right Grant
- 1999-11-08 EP EP99956367A patent/EP1194481B1/en not_active Expired - Lifetime
- 1999-11-08 PL PL348185A patent/PL196537B1/en unknown
- 1999-11-08 CA CA002349489A patent/CA2349489C/en not_active Expired - Fee Related
- 1999-11-08 CN CNB998130923A patent/CN1134493C/en not_active Expired - Fee Related
- 1999-11-08 CZ CZ20011614A patent/CZ298481B6/en not_active IP Right Cessation
- 1999-11-08 JP JP2000581084A patent/JP3709342B2/en not_active Expired - Fee Related
- 1999-11-08 KR KR10-2001-7005850A patent/KR100407717B1/en not_active IP Right Cessation
- 1999-11-08 HU HU0104344A patent/HU227716B1/en not_active IP Right Cessation
- 1999-11-08 AU AU12991/00A patent/AU1299100A/en not_active Abandoned
- 1999-11-08 AT AT99956367T patent/ATE301687T1/en not_active IP Right Cessation
- 1999-11-08 BR BR9915156-1A patent/BR9915156A/en not_active IP Right Cessation
- 1999-11-08 RU RU2001116124/04A patent/RU2201425C2/en not_active IP Right Cessation
-
2001
- 2001-04-23 NO NO20011988A patent/NO327394B1/en not_active IP Right Cessation
Non-Patent Citations (1)
Title |
---|
See references of WO0027911A1 * |
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US7197060B2 (en) | 2003-05-02 | 2007-03-27 | Videojet Technologies | Waveguide laser |
US7230967B2 (en) | 2003-05-02 | 2007-06-12 | Videojet Technologies | Waveguide laser |
Also Published As
Publication number | Publication date |
---|---|
HU227716B1 (en) | 2012-01-30 |
CA2349489A1 (en) | 2000-05-18 |
CN1134493C (en) | 2004-01-14 |
NO20011988D0 (en) | 2001-04-23 |
ATE301687T1 (en) | 2005-08-15 |
BR9915156A (en) | 2001-08-07 |
AU1299100A (en) | 2000-05-29 |
ES2247839T3 (en) | 2006-03-01 |
HUP0104344A2 (en) | 2002-03-28 |
EP1194481B1 (en) | 2005-08-10 |
RU2201425C2 (en) | 2003-03-27 |
PL348185A1 (en) | 2002-05-06 |
DE69926664D1 (en) | 2005-09-15 |
RU2001116124A (en) | 2004-02-20 |
DE69926664T2 (en) | 2006-08-24 |
CZ20011614A3 (en) | 2001-11-14 |
NO985211L (en) | 2000-05-10 |
KR100407717B1 (en) | 2003-12-03 |
CZ298481B6 (en) | 2007-10-17 |
KR20010100997A (en) | 2001-11-14 |
JP2002529560A (en) | 2002-09-10 |
PL196537B1 (en) | 2008-01-31 |
HUP0104344A3 (en) | 2003-05-28 |
JP3709342B2 (en) | 2005-10-26 |
NO309484B1 (en) | 2001-02-05 |
CN1325421A (en) | 2001-12-05 |
US6809144B1 (en) | 2004-10-26 |
NO20011988L (en) | 2001-04-23 |
NO327394B1 (en) | 2009-06-22 |
WO2000027911A1 (en) | 2000-05-18 |
CA2349489C (en) | 2006-01-10 |
NO985211D0 (en) | 1998-11-09 |
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